High-speed measurement of rotational anisotropy nonlinear optical harmonic generation using position-sensitive detection.

We present a method of performing high-speed rotational anisotropy nonlinear optical harmonic generation experiments at rotational frequencies of several hertz by projecting the harmonic light reflected at different angles from a sample onto a stationary position-sensitive detector. The high rotational speed of the technique, 10(3) to 10(4) times larger than existing methods, permits precise measurements of the crystallographic and electronic symmetries of samples by averaging over low frequency laser-power, beam-pointing, and pulse-width fluctuations. We demonstrate the sensitivity of our technique by resolving the bulk fourfold rotational symmetry of GaAs about its [001] axis using second-harmonic generation.